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Title: Regioselective atomic layer deposition in metal–organic frameworks directed by dispersion interactions

Abstract

The application of atomic layer deposition (ALD) to metal–organic frameworks (MOFs) offers a promising new approach to synthesize designer functional materials with atomic precision. While ALD on flat substrates is well established, the complexity of the pore architecture and surface chemistry in MOFs present new challenges. Through in situ synchrotron X-ray powder diffraction, we visualize how the deposited atoms are localized and redistribute within the MOF during ALD. We demonstrate that the ALD is regioselective, with preferential deposition of oxy-Zn(II) species within the small pores of NU-1000. As a result, complementary density functional calculations indicate that this startling regioselectivity is driven by dispersion interactions associated with the preferential adsorption sites for the organometallic precursors prior to reaction.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1339610
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 41; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gallington, Leighanne C., Kim, In Soo, Liu, Wei-Guang, Yakovenko, Andrey A., Platero-Prats, Ana E., Li, Zhanyong, Wang, Timothy C., Hupp, Joseph, Farha, Omar K., Truhlar, Donald G., Martinson, Alex B. F., and Chapman, Karena W. Regioselective atomic layer deposition in metal–organic frameworks directed by dispersion interactions. United States: N. p., 2016. Web. doi:10.1021/jacs.6b08711.
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Gallington, Leighanne C., Kim, In Soo, Liu, Wei-Guang, Yakovenko, Andrey A., Platero-Prats, Ana E., Li, Zhanyong, Wang, Timothy C., Hupp, Joseph, Farha, Omar K., Truhlar, Donald G., Martinson, Alex B. F., & Chapman, Karena W. Regioselective atomic layer deposition in metal–organic frameworks directed by dispersion interactions. United States. https://doi.org/10.1021/jacs.6b08711
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Gallington, Leighanne C., Kim, In Soo, Liu, Wei-Guang, Yakovenko, Andrey A., Platero-Prats, Ana E., Li, Zhanyong, Wang, Timothy C., Hupp, Joseph, Farha, Omar K., Truhlar, Donald G., Martinson, Alex B. F., and Chapman, Karena W. Mon . "Regioselective atomic layer deposition in metal–organic frameworks directed by dispersion interactions". United States. https://doi.org/10.1021/jacs.6b08711. https://www.osti.gov/servlets/purl/1339610.
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@article{osti_1339610,
title = {Regioselective atomic layer deposition in metal–organic frameworks directed by dispersion interactions},
author = {Gallington, Leighanne C. and Kim, In Soo and Liu, Wei-Guang and Yakovenko, Andrey A. and Platero-Prats, Ana E. and Li, Zhanyong and Wang, Timothy C. and Hupp, Joseph and Farha, Omar K. and Truhlar, Donald G. and Martinson, Alex B. F. and Chapman, Karena W.},
abstractNote = {The application of atomic layer deposition (ALD) to metal–organic frameworks (MOFs) offers a promising new approach to synthesize designer functional materials with atomic precision. While ALD on flat substrates is well established, the complexity of the pore architecture and surface chemistry in MOFs present new challenges. Through in situ synchrotron X-ray powder diffraction, we visualize how the deposited atoms are localized and redistribute within the MOF during ALD. We demonstrate that the ALD is regioselective, with preferential deposition of oxy-Zn(II) species within the small pores of NU-1000. As a result, complementary density functional calculations indicate that this startling regioselectivity is driven by dispersion interactions associated with the preferential adsorption sites for the organometallic precursors prior to reaction.},
doi = {10.1021/jacs.6b08711},
journal = {Journal of the American Chemical Society},
number = 41,
volume = 138,
place = {United States},
year = {Mon Oct 03 00:00:00 EDT 2016},
month = {Mon Oct 03 00:00:00 EDT 2016}
}
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Publisher's Version of Record
https://doi.org/10.1021/jacs.6b08711
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    Works referencing / citing this record:

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